Southern Hemispheric halon trends (1978-1998) and global halon emissions

Southern hemispheric data (1978-1998) on four halons are reported. Halon-derived bromine increased by a factor of 10 from 0.6–0.7 parts per trillion (ppt) in 1978 to more than 7 ppt in early 1998, currently growing at 3% yr−1. In 1997 the mixing ratios were 4.0 (CBrClF2, H-1211), 2.1 (CBrF3, H-1301), 0.4 (CBrF2CBrF2, H-2402), and 0.04 ppt (CBr2F2, H-1202), contributing ∼60, 30, 10 and 1% respectively to halon-derived bromine (40% of background tropospheric bromine). The halons exhibit different growth patterns: CBrClF2 continues linearly (0.20 ppt yr−1), CBrF3 slows significantly (0.03 ppt yr−1, early 1998), CBrF2CBrF2 stops and CBr2F2 increases (17% yr−1 in early 1998). CBr2F2 shows a photochemically driven annual cycle. CBrClF2 and CBrF3 emissions (1963–2100) have been estimated from past and future production figures, in developed and developing countries, and from release estimates from the various halon banks. Mixing ratios have been calculated from a two-dimensional model incorporating seasonal transport and halon photochemistry and a latitudinal source function. The model-derived atmospheric lifetimes are 17 (CBrClF2), 62 (CBrF3), 20 (CBrF2CBrF2), and 2.9 (CBr2F2) years. Calculated and measured mixing ratios of CBrF3 agree reasonably but not for CBrClF2 in recent years. The model has been used to derive independently halon emissions that are consistent with the observed atmospheric trends. The continued growth of CBrClF2 in the background atmosphere could be due to enhanced production and emission in the Peoples' Republic of China, which may also explain the recent acceleration in growth of CBr2F2, a by-product of CBrClF2 manufacture. The recent atmospheric growth of CBr2F2 may also be due to increased direct usage. The expected long-term recovery of stratospheric ozone could be delayed if the current halon growth continues into the next decade.

[1]  Jürgen M. Lobert,et al.  Growth and distribution of halons in the atmosphere , 1998 .

[2]  James W. Elkins,et al.  Decline in the Tropospheric Abundance of Halogen from Halocarbons: Implications for Stratospheric Ozone Depletion , 1996, Science.

[3]  S. Schauffler,et al.  Measurements of bromine containing organic compounds at the tropical tropopause , 1998 .

[4]  A. Hough The development of a two-dimensional global tropospheric model—1. The model transport , 1989 .

[5]  Donald J. Wuebbles,et al.  Ozone depletion and chlorine loading potentials , 1991 .

[6]  R. Derwent,et al.  Measurement of CCl3F and CCl4 at Harwell over the period January 1975–November 1977 , 1979 .

[7]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[8]  W. Sturges,et al.  Growth of fluoroform (CHF3, HFC‐23) in the background atmosphere , 1998 .

[9]  James B. Burkholder,et al.  Atmospheric fate of CF3Br, CF2Br2, CF2ClBr, and CF2BrCF2BR , 1991 .

[10]  E. Atlas,et al.  Alkyl nitrates, nonmethane hydrocarbons, and halocarbon gases over the equatorial Pacific Ocean during Saga 3 , 1993 .

[11]  R. Weiss,et al.  GAGE/AGAGE measurements indicating reductions in global emissions of CCl3F and CCl2F2 in 1992–1994 , 1997 .

[12]  M. McCormick,et al.  Ozone response to enhanced heterogeneous processing after the eruption of Mt. Pinatubo , 1994 .

[13]  S. Lal,et al.  Increasing abundance of CBrClF2 in the atmosphere , 1985, Nature.

[14]  A. Ravishankara,et al.  Kinetics of O(1D) reactions with bromocarbons , 1993 .

[15]  Stuart A. Penkett,et al.  Recent tropospheric growth rate and distribution of HFC-134a (CF3CH2F) , 1996 .

[16]  James W. Elkins,et al.  Observations of HFC‐134a in the remote troposphere , 1996 .

[17]  L. Heidt,et al.  Brominated organic species in the Arctic atmosphere , 1984 .

[18]  M. Rycroft,et al.  An interhemispheric comparison of the concentrations of bromine compounds in the atmosphere , 1985, Nature.

[19]  D. M. Cunnold,et al.  Atmospheric Trends and Lifetime of CH3CCI3 and Global OH Concentrations , 1995, Science.

[20]  Stuart A. Penkett,et al.  Measurements of HCFC‐142b and HCFC‐141b in the Cape Grim air Archive: 1978–1993 , 1995 .

[21]  P. Fabian,et al.  Halocarbons in the stratosphere , 1981, Nature.

[22]  A. Mcculloch Global production and emissions of bromochlorodifluoromethane and bromotrifluoromethane (halons 1211 and 1301) , 1992 .

[23]  D. Weisenstein,et al.  Distribution of halon-1211 in the upper troposphere and lower stratosphere and the 1994 total bromine budget , 1998 .

[24]  S. Lal,et al.  Measurements of atmospheric BrOx radicals in the tropical and mid-latitude atmosphere , 1988, Nature.

[25]  R. Weiss,et al.  Global trends and emission estimates of CCl4 from in situ background observations from July 1978 to June 1996 , 1998 .

[26]  M. Khalil,et al.  Atmospheric measurements of CF4 and other fluorocarbons containing the CF3 grouping , 1981 .

[27]  S. Solomon,et al.  Measurements of halogenated organic compounds near the tropical tropopause , 1993 .

[28]  S. Wofsy,et al.  Chemical Loss of Ozone in the Arctic Polar Vortex in the Winter of 1991-1992 , 1993, Science.

[29]  P. Fraser,et al.  Methane, carbon monoxide and methylchloroform in the southern hemisphere , 1986 .

[30]  James W. Elkins,et al.  Early trends in the global tropospheric abundance of hydrochlorofluorocarbon-141b and 142b , 1994 .

[31]  R. Weiss,et al.  Lifetime and emission estimates of 1,1,2-trichlorotrifluorethane (CFC-113) from daily global background observations , 1996 .

[32]  S. Montzka,et al.  A decrease in the growth rates of atmospheric halon concentrations , 1992, Nature.

[33]  M. Khalil,et al.  Gaseous bromine in the Arctic and Arctic haze , 1984 .

[34]  I. Isaksen,et al.  Global distribution of sulfur compounds in the troposphere estimated in a height/latitude transport model , 1980 .

[35]  D. Gillotay,et al.  Ultraviolet absorption spectrum of trifluoro-bromo-methane, difluoro-dibromo-methane and difluoro-bromo-chloro-methane in the vapor phase , 2018 .

[36]  R. Weiss,et al.  Global trends and annual releases of CCl3F and CCl2F2 estimated from ALE/GAGE and other measurements from July 1978 to June 1991 , 1994 .

[37]  M. Mills,et al.  On the age of stratospheric air and ozone depletion potentials in polar regions , 1992 .

[38]  R. A. Plumb,et al.  The Zonally Averaged Transport Characteristics of the GFDL General Circulation/Transport Model , 1987 .

[39]  J. Dymond,et al.  The Virial Coefficients of Pure Gases and Mixtures: A Critical Compilation , 1979 .

[40]  P. Fraser,et al.  Trends in source gases , 1989 .

[41]  A. Hough Development of a two-dimensional global tropospheric model: Model chemistry , 1991 .

[42]  D. Toohey,et al.  Kinetics of O3 destruction by ClO and BrO within the Antarctic vortex: An analysis based on in situ ER‐2 data , 1989 .

[43]  H. Singh,et al.  Selected man‐made halogenated chemicals in the air and oceanic environment , 1983 .